The main objective is to determine compositional and structural details of the inorganic phase in teeth and bones. Infrared and Raman spectroscopy, x-ray diffraction and chemical methods are employed in these studies. Methods are devised for the preparation of synthetic calcium apatites having controlled physical properties (crystal size and perfection) and chemical constituents (hydroxide, fluoride, chloride, carbonate, water, acid phosphate and other ions). The vibrational spectra of these apatites and related compounds are assigned and characterized. Isotopically enriched apatite analogs are prepared to facilitate spectral assignments. The spectroscopic assignments and supplemental spectral data (temperature dependence and polarization) are then utilized to establish compositional and structural details of the apatites in question, which include: the type and geometry of constituent ions; the site or number of sites occupied by the ions; orientation of ions; chemical bonding and interactions of ions; and semi-quantitative estimations of the constituents present. The results for these controlled apatite systems are then related to the inorganic phase in calcified tissues. Combined infrared, Raman, and x-ray diffraction methods were used to identify and semi-qualify phases and structural forms of calcium phosphate substances formed upon coating titanium implant surfaces by plasma spraying from hydroxyapatite sources. A large quantity, about one kg, of hydroxyapatite previously prepared from solution, was analyzed in detail by numerous physicochemical methods. This hydroxyapatite was found suitable to be certified as a Standard Reference Material, and it will be available at a future date from NIST.